活性位点电子密度变化对光催化CO2活化和选择转化的影响

doi:10.3866/PKU.WHXB202303029

物理化学学报 >> 2024, Vol. 40 >> Issue (1): 2303029.doi: 10.3866/PKU.WHXB202303029

活性位点电子密度变化对光催化CO₂活化和选择转化的影响

曹玥晗¹^,², 郭瑞², 马敏智², 黄泽皑², 周莹¹^,²^,*()

¹ 西南石油大学油气藏地质及开发工程国家重点实验室, 成都 610500
² 西南石油大学新能源与材料学院, 成都 610500

收稿日期:2023-03-14 录用日期:2023-04-14 发布日期:2023-08-21
通讯作者: 周莹 E-mail:yzhou@swpu.edu.cn
作者简介:第一联系人：
^†These authors contributed equally to this work.
基金资助:
国家自然科学基金(22209135);中央引导地方科技发展资金项目(22ZYZYTS0231);中国博士后科学基金(2022M722635);四川省自然科学基金(2022NSFSC1264);四川省博士后创新人才支持项目;四川省科技项目(2021ZYD0035);四川省科技项目(2022YFH0084);四川省科技项目(2021YFH0055);四川省科技项目(2022YFSY0050)

Effects of Electron Density Variation of Active Sites in CO₂ Activation and Photoreduction: A Review

Yuehan Cao¹^,², Rui Guo², Minzhi Ma², Zeai Huang², Ying Zhou¹^,²^,*()

¹ State Key Laboratory of Oil and Gas Reservoir Geology and Exploitation, Southwest Petroleum University, Chengdu 610500, China
² School of New Energy and Materials, Southwest Petroleum University, Chengdu 610500, China

Received:2023-03-14 Accepted:2023-04-14 Published:2023-08-21
Contact: Ying Zhou E-mail:yzhou@swpu.edu.cn
Supported by:
the National Natural Science Foundation of China(22209135);Special Project for the Central Government to Guide the Development of Local Science and Technology in Sichuan Province(22ZYZYTS0231);China Postdoctoral Science Foundation(2022M722635);Natural Science Foundation of Sichuan Province(2022NSFSC1264);Sichuan Province Innovative Talent Funding Project for Postdoctoral Fellows;Sichuan Science and Technology Program(2021ZYD0035);Sichuan Science and Technology Program(2022YFH0084);Sichuan Science and Technology Program(2021YFH0055);Sichuan Science and Technology Program(2022YFSY0050)

摘要/Abstract

摘要：

光催化二氧化碳(CO₂)还原制液体燃料和高值化学品技术不仅能充分利用可再生能源太阳光，实现化学储能；更重要的是，此技术以温室气体CO₂为原料，因此可以减缓全球温室效应，构造人工碳循环。然而，光催化CO₂还原制液体燃料和高值化学品反应过程中面临诸多挑战：(1) CO₂分子吸附和活化过程困难；(2) (高附加值)碳产物选择性低；(3)产物生成后易发生其他副反应导致催化剂失活或产物选择性下降。受到以上三个挑战的制约，目前的反应效率较低，难以满足工业化应用。由于光催化CO₂向高值化学品的转化过程为质子耦合光生电子参与的还原反应，因此活性位点的电子密度会显著影响以上挑战的解决。然而，光催化CO₂还原过程涉及众多基元步骤，每个基元步骤对于活性位点的电子密度要求并不清晰，这导致无法有针对性设计高效的催化剂来促进光催化CO₂分子的有效活化及高选择性转化。本文综述了近期活性位点的电子密度变化对于CO₂分子吸附和活化过程、碳产物选择性调控和产物脱附及过氧化的影响规律，并总结了调控活性位点上电子密度的方法，旨在对未来设计高效光催化剂提供参考和理论依据。

关键词: 光催化二氧化碳还原, 高附加值化学品, 电子密度调控, 活性位点, 产物选择性

Abstract:

Photocatalytic reduction of CO₂ into value-added chemicals is a feasible approach to harvest solar light energy and storing energy in the form of chemical fuels as well as to mitigate the effects of global climate change and help achieve an artificial carbon cycle. However, the efficiency of CO₂ photoreduction is low for commercial purposes. This is mainly due to the difficult adsorption and activation process of CO₂ molecules, the unsatisfactory selectivity of target products, and the uncontrolled-subsequent reaction process of the generated carbon products. CO₂ photoreduction requires substantial electrons for participation. Hence, these issues are due to the electron density modulation of the active sites of catalysts. Unfortunately, the CO₂ photoreduction process involves multi-fundamental steps, which leads to different requirements in electron density modulation. The performance might not be effectively improved by directly enhancing or weakening the total electron density of active sites. In this paper, we summarize recent advances in the influence of electron density variation of the active sites in strengthening the adsorption and activation of CO₂ molecules, enhancing the selectivity of target carbon products and modulating the subsequent reaction process of the generated carbon products. This review begins with the effect of different types of active sites in strengthening the adsorption and activation of the CO₂ molecules and the related methods for modulating the electron density of active sites. Active sites with high electron densities can significantly enhance the adsorption and activation of CO₂. Introducing metal and fabricating the defects on catalyst surfaces are effective strategies for fabricating the electron-rich active sites. After that, we discuss the influence of electron density variation in enhancing the selectivity of target carbon products in detail. In this part, the related effects in the multielectron donation from the catalyst surface, the reactive intermediates, and the competition hydrogen evolution reaction are summarized. Enhancing the electron density of active sites strengthens the former two processes. For multielectron donation, introducing cocatalysts or fabricating heterostructures are the most effective methods for enhancing the electron density of active sites. The adsorption and conversion process of intermediates are mainly affected by the accumulation sites of electrons. The active sites with low coordination are more favorable to achieving the generation of multi-electronic carbon products. In contrast, the hydrogen evolution reaction is significantly inhibited by reducing the electron density of active sites. Moreover, elemental doping is considered one of the most effective strategies. Finally, we describe the method for weakening the electron density of active sites to promote product desorption and inhibit the photooxidation of reactive products.

Key words: CO₂ photoreduction, Value-added chemicals, Electron density modulation, Active sites, Product selectivity

曹玥晗, 郭瑞, 马敏智, 黄泽皑, 周莹. 活性位点电子密度变化对光催化CO₂活化和选择转化的影响[J]. 物理化学学报, 2024, 40(1), 2303029. doi: 10.3866/PKU.WHXB202303029

Yuehan Cao, Rui Guo, Minzhi Ma, Zeai Huang, Ying Zhou. Effects of Electron Density Variation of Active Sites in CO₂ Activation and Photoreduction: A Review[J]. Acta Phys. -Chim. Sin. 2024, 40(1), 2303029. doi: 10.3866/PKU.WHXB202303029

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202303029

https://www.whxb.pku.edu.cn/CN/Y2024/V40/I1/2303029

图/表 9

Table 1

Recent improvement of CO2 photoreduction by modulating the surface electron density."

Photocatalysts	Modification methods	Variation of surface electron density	Original product generation rate (μmol∙g⁻¹∙h⁻¹)	Modified product generation rate (μmol∙g⁻¹∙h⁻¹)	Original product selectivity (%)	Modified product selectivity (%)	References
BOC and BOC-VDWGs-AL	Delamination	Increase	CO: 9.5	CO: 188.2	–	–	70
Bi₄O₅Cl₂ and V_Cl-Bi₄O₅Cl₂	Defects	Decrease	CO: 0.0	CO: 14.6	–	–	77
NiO and Er/NiO_1−x	Cocatalysts	Increase	CO: 14	CO: 368	–	–	72
BiOBr and Bi-MOF	Heterojunction	Decrease	CO: 5.1	CO: 22.0	–	–	73
ZnSe QDs and ZnSe/CdS DORs	Heterojunction	Decrease	CO: 0.0	CO: 11.3	–	--	74
ROH-NiCo₂O₃ and Cu₂S@ROH-NiCo₂O₃	Heterojunction	Increase	CO: 1178.0 H₂: 461.0	CO: 7067.0 H₂: 2767.0	CO: 42.0	CO: 72	78
CdS and CdS/EDA	Heterojunction	Increase	CO: 2.9 H₂: 62.9	CO: 115.6 H₂: 959.4	–	–	63
U-Cu₂O-LTH@PCN-3 and PCN	Heterojunction	Increase	CH₃OH: 48.9	CH₃OH: 4.7	–	–	61
Pb_0.6Bi_1.4Cs_0.6O₂Cl₂ and Pb_0.6Bi_1.4O₂Cl_1.4	Delamination	Increase	CH₃OH: 6.6 CO: 4.5	CH₃OH: 0.9 CO: 0.6	–	–	65
CN and mCD/CN	Heterojunction	Increase	CH₃OH: 0.0 CO: 0.0	CH₃OH: 13.9 CO: 0.1	–	–	68
CdS and CdS/A-GO	Heterojunction	Increase	CO: 0.6 H₂: 5.1 CH₃OH: 0.1	CO: 2.2 H₂: 76.3 CH₃OH: 26.5	–	–	67
BiOBr and 20%CdS/BiOBr	Heterojunction	Decrease	CH₃OH: 104.3	CH₃OH: 219.0	–	–	75
In₂O₃ and N-In₂O₃	Doping	Decrease	CO: 0.0	CH₃OH: 394.0 CH₄: 0.1 CO: 230	–	–	76
CeO₂ and Pd/CeO₂	Cocatalysts	Increase	CH₃OH: 12.7	CH₄: 41.6	CH₄: 9	CH₄: 100	62
Cd_1−xS and Au_SA/Cd_1−xS	Cocatalysts	Increase	CO: 0.1 CH₄: 0.2 H₂: 0.0	CO: 32.2 CH₄: 11.3 H₂: 7.9	–	–	59
BMO and BMO-R	Defects	Increase	CO: 17.7 CH₄: 3.3	CO: 61.5 CH₄: 12.4	–	–	60
BiOBr and La/BiOBr	Cocatalysts	Increase	CH₃OH: 10.6	CH₃OH: 21.0 CO: 0.1 CH₄: 1.6	CH₃OH: 100	CH₃OH: 92	66
Pd₁/C₃N₄ and Pd_1+NPs/C₃N₄	Cocatalysts	Increase	CH₄: 4.2 CO: 10.3	CH₄: 20.3 CO: 0.8	CH₄: 55	CH₄: 97	69
Cu₃SnS₄ and V_S Cu₃SnS₄	Defects	Increase	CH₄: 5.6 CO: 16.3	CH₄: 22.7 CO: 18.4	–	–	71
TiO₂ and V_Ti-TiO₂	Defects	Increase	CH₄: 15.7	CH₄: 28.3	CH₄: 34	CH₄: 97	79
Co₃O₄ and V_O-Co₃O₄/NiCo₂O₄	Heterojunctionand Defects	Increase	CO: 11.2	CH₄: 20.3	–	–	80
C₃N₄ and Co/C₃N₄	Cocatalysts	Increase	CH₃OH: 17.7	CH₃OH: 235.5 H₂: 18.9 CO: 2.9 CH₄: 3.4 C₂H₄: 1.1 C₃H₆: 1.4 CH₃OCH₃: 3.3	CH₃OH: 100	CH₃OH: 96	64

Table 1

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Fig 6

Fig 7

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活性位点电子密度变化对光催化CO₂活化和选择转化的影响

Effects of Electron Density Variation of Active Sites in CO₂ Activation and Photoreduction: A Review

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